Novel luminescent organogelators based on nucleoside functionalized with carbazole (UC8, UC12 and UC16) were designed and synthesized. Their gelation ability was tested and it was found that both UC12 and UC16 could form stable organogels in toluene/petroleum ether. The UV‐vis absorption, fluorescence emission and IR spectral changes during the gelation of UC12 proved that the self‐assembly was driven by H‐bonding. The morphology of the xerogel UC16 obtained from toluene/petroleum ether (v/v = 1/1) displayed tough rod‐like microstructures, and 3D networks formed from lots of nanofibers were observed for the xerogel UC16 obtained from toluene/petroleum ether (v/v = 2/1). It was interesting that the obtained organogels emitting blue light could be destroyed by the addition of F‐, accompanied with the declining the emission intensity. Therefore, these organogels could be used as sensory materials to recognize F‐.